American Journal of Applied Sciences 9 (6): 946-954, 2012

ISSN 1546-9239
2012 Science Publications
Corresponding Author: Mikrajuddin Abdullah, Department of Physics, Faculty of Mathematics and Natural Science,
Bandung Institute of Technology Jalan Ganeca 10, Bandung 40132 Indonesia
946

A General Formula for Ion Concentration-
Dependent Electrical Conductivities in Polymer Electrolytes

1
Mahardika Prasetya Aji,
1
Masturi,
2
Satria Bijaksana,
1
Khairurrijal and
1
Mikrajuddin Abdullah
1
Department of

Physics, Faculty of Mathematics and Natural Science,
2
Department of Global Geophysics, Faculty of Mining and Petroleum Engineering,
Bandung Institute of Technology Jalan Ganeca 10, Bandung 40132, Indonesia

Abstract: Problem statement: The aim of this study is to develop a model for describing the effect of
ion concentration on the electrical conductivity of polymer electrolytes by considering two mechanisms
simultaneously: Enhancements of ion concentration and amorphous phase. Approach: The problems
based on new observations in polymer electrolyte when ion concentration in the polymer electrolytes was
increased, both the fraction of amorphous phase and the charge carriers increase simultaneously. The
model was based on the assumption when ions were inserted into the polymer host, there was an
optimum distance between ions at which the ions move easily throughout the polymer. The average
distance between ions in the polymer depends on the ion concentration. And we also considered the effect
of ion concentration on the amorphous phase in the polymer. Results: We inspected the validity of the
model by comparing the model predictions with various experimental data. The new analytical
expressions for the electrical conductivity dependent of ion concentration was developed by considering
two mechanisms simultaneously in polymer electrolytes, i.e., enhancement of the carries concentration
and amorphous phase fraction. Interestingly, most of fitting parameters were not arbitrarily selected, but
were derived from the appropriate experimental data. Conclusion: The model can be used to explain the
conductivity behavior of other polymer electrolyte systems by selecting appropriately less number of
parameters. This model result is fully supported by available experimental data.

Key words: Electrical conductivity, polymer electrolyte, ion concentration effect, experimental data,
amorphous phase, increase simultaneously

INTRODUCTION

The dependence of electrical conductivity of
polymer electrolytes onion concentration has been well
known. The conductivity initially increases with ion
concentration, reaches the maximum at a certain
concentration after which it turns down at high ion
concentrations (Khiar and Arof, 2011; Gong et al.,
2008; Kang and Fang, 2004; Rajendran et al., 2003;
Kang et al., 2003; Xu et al., 2001).
Many explanations have been exposed to explain
these observations. At low concentrations the
conductivity increases due to increasing in the charge
carriers, while at high concentrations, repulsion
between ions at short distances inhibits the transport of
ions to weaken the conductivity.
New observations on this topic are interesting to be
discussed (Aji et al., 2012; Bhargav et al., 2010; 2007a;
2007b; Mohamad et al., 2003). When ion concentration
in the polymer electrolytes is increased, both the
fraction of amorphous phase and the charge carriers
increase simultaneously.



Fig. 1: Increasing the ion concentration will increase the
carrier concentration and the fraction of amorphous
phase
Am. J. Applied Sci., 9 (6): 946-954, 2012

947
The ion concentration does not affect only the charge
carriers, but also the structure of the polymer host from
crystalline to amorphous. Therefore, a theory for
explaining the electrical conductivity development due
to insertion of ions must consider the occurrence of
these two mechanisms.
The aim of this study is to develop a model for
describing the effect of ion concentration on the electrical
conductivity of polymer electrolytes by considering two
mechanisms simultaneously: Enhancements of ion
concentration and amorphous phase (see illustration in
Fig. 1). The predictions of the model were compared to
experimental data reported by many authors (Aji et al.,
2012; Amir et al., 2011; Noor et al., 2010; Bhargav et
al., 2009; Hirankumar et al., 2006).

MATERIALS AND METHODS

The model was based on the assumption when ions
are inserted into the polymer host, there is an optimum
distance between ions at which the ions move easily
throughout the polymer. This distance corresponds to
the lowest energy for ion hopping. If ion distances are
shorter, repulsion between ions might cause a reduction
in the electrical conductivity. On the other hand, when
the ion distances are too far, a long distance hopping is
required to generate the conductivity, which implies the
reduction in the conductivity too. If the distance
between ions at a specific concentration is , the
interaction energy experiences by an ion can be
expressed in the Taylor series as Eq. 1:

( ) ( ) ( )
( ) ( )
0
0
0
2
0 0 2
1
1
3
3
2
0 0 3
1
dE 1 d E
E l = E l + l - l +
dl 2 dl
1 d E
l - l + l - l + ...
6 dl
(1)

with
0
is the optimum distance as mentioned above. Since
at
0
, dE/d|
0
= 0, we obtain the deviation of energy from
the energy when the ions are separated by
0
as Eq. 2:

( ) ( ) ( ) ( )
( )
0
0
2
2
0 0 2
1
3
3
0 3
1
1 d E
E l = E l - E l = l - l
2 dl
1 d E
+ l - l + ...
6 dl
(2)

Actually, the distances between ions in the polymer
host are not equal. The ion positions distribute
randomly, ranging from the shortest to the longer ones.
Therefore, it is more accurate if we introduce a
probability function to explain the distance distribution.
Since the distances are always positive, the proper
distribution function for explaining this distance is the
log normal distribution. This selection can be
compared to selection of the log normal distribution
for explaining size distribution of particles (Chen et
al., 2009; Hafraoui et al., 2008; Berret et al., 2007;
Feng and Bertelo, 2004; Teraoka, 2002). The particle
sizes are never negative so that the log normal
distribution is the best function to explain it.
Suppose the distribution density of ion distances
separated by is (). The fraction on ions that are
separated by distances between and + d are Eq.
3 (Mikrajuddin et al., 2001):

( ) av
2
ln ln / 2
1
f ( )d e d
2

=

(3)

With
av
is the average distance between ions and
is the geometrical standard deviation. The average
deviation of energy for ion hopping is Eq. 4:

0
0
2
av 2
0
3
2 3
0 0 3
0 0
1 d E
E( ) E( )f ( )d
2 d
1 d E
( ) f ( )d ( ) f ( )d ...
6 d

= =

+ +

(4)

If S is the change in entropy relative to the
entropy when all ions are separated by
0
, the
expression for the free energy change is F(
av
) =
E(
av
)-TS. The probability of ion hopping caused by
ion concentration will be proportional to Eq. 5:

S/ k av av
hop
F( )
E( )/kT
P exp e e
kT

| |

|
\

(5)

We also considered the effect of ion concentration
on the amorphous phase in the polymer. We assumed
the amorphous phase is composed of a large number of
islands (Fig. 2) with an average size L.
In the amorphous phase, the ions are very mobile.
We assumed the ions diffuse in one-dimensional
cages bounded by [L/2, +L/2] and are absorbed
when reaching the cage wall. The cage corresponds to
the amorphous island and the wall corresponds to the
boundary between amorphous and crystalline phases.
We determined the survival probability of the ions in
the amorphous phase and assumed this probability
controls the ionic conductivity.
Am. J. Applied Sci., 9 (6): 946-954, 2012

948


Fig. 2: The amorphous phase was assumed to be
composed of amorphous islands of average size L

The survival probability of ions in the amorphous
phase satisfies Eq. 6 (Krapivsky and Redner, 1996):

( ) ( )
L 2
L 2
S t C x, t dx
+

=

(6)

where, C(x, t) is the ionic concentration at position x
and at time t. The ion concentration evolves according
to the diffusion Eq. 7:

( ) ( )
2
2
C x, t C x, t
D
t x

=

(7)

With D is the diffusion coefficient. Since the ions
are absorbed by the cage wall, the ion concentration
satisfies the boundary condition of C (L/2, t) = 0.
The survival probability of an ion may be obtained
by integration of ion concentration over the region. For
simplicity, we assumed the initial concentration was
homogeneously distributed or C (x, 0) = L, with is a
constant. Using both the boundary and the initial
condition we obtained the following solution for the ion
concentration Eq. 8 (Krapivsky and Redner, 1996):

( )
2 2 2
D n t L
n
n 1
n
C x, t A sin x e
L

=
| |
=
|
\
(8)

With
L
n
0
2 n
A sin x dx
L L L
| | | |
=

| |
\ \
Assuming that the first
term in Eq. 8 is very dominant, we can approximate Eq. 9:

( )
2 2
D t L
4
C x, t sin x e
L L

| |

|
\
(9)

Indeed, the ratio of the first to the second terms is
proportional to
2 2
exp(3D t / L ) . The survival probability
is then Eq. 10:

( )
L 2
2 2
D t L
L 2
4
S t e sin x dx
L L
+

| |
=

|
\
(10)
And the time average of the survival probability
can be written as Eq. 11:

( )
2 2
S t e D L
c
(11)

where,
c
is referred to the characteristic time and might
be related to the relaxation time of polymer segmental
motion in the amorphous phase. The motion of ions in
the amorphous phase is assisted by this segmental
motion (Vogel, 1921; Li et al., 2008; Fonseca et al.,
2007; Xu et al., 2001; Noda and Watanabe, 2000).
We assumed the second term in Eq. 4 is much
smaller than the first term. Since we dont have data of
the distance distribution of ions, at present we assumed
the ions are separated equally so that we can replace the
distribution function as a Dirac delta
function,
av
( ) and finally found that Eq. 12:

0
2 2 2
1/ 2d E/ d ( ) / kT
av 0
S/ k
hop
P e e

(12)

The average distance between ions in the
polymer depends on the ion concentration. If C is the
ion concentration (number per unit of volume) we
may write
1/ 3
av
1/ C = and the probability of ion
hopping becomes Eq. 13 and 14:

S/ k 1/ 3 1/ 3 2
hop 0
P e exp (1/ C 1/ C )

(

(13)

With:

0
2
2
1 d E
2kT d
=

(14)

We speculated that the size of amorphous islands
is proportional to the fraction of amorphous phase.
This assumption is valid when the number of
amorphous islands remains constant as the ion
concentration is varied. Taking this assumption as a
very rough approximation, we obtain a relation L
2
=

2

a
2/3
, where
a
is the fraction of amorphous phase
and is a constant. Since
a
is in the order of unity,
the value of approaches L. The average survival
probability becomes Eq. 15 and 16:

( ) ( )
2 3
a
S t exp v

(15)

With:

2
c
2
D
=

(16)
Am. J. Applied Sci., 9 (6): 946-954, 2012

949
Since the electrical conductivity depends
simultaneously on ion concentration and amorphous
phase fraction, a general expression for the electrical
conductivity satisfies Eq. 17:

( )
2
1 3 1 3
2 3 1 C 1 C
v 0
a
0
e e

= (17)

With
0
is a constant for a specific polymer
electrolyte.
We inspected the validity of the above model by
comparing the model predictions with various
experimental data. At present we compared the model
with the conductivity data of PVA, PEO and PEMA
based polymer electrolytes containing different ions such
as PVA.NaF (Bhargav et al., 2009), PVA.LiOH (Aji et
al., 2012), PVA.AgNO
3
(Hirankumar et al., 2006) and
PEO.LiCF
3
SO
3
with plasticizer ENR50 (Noor et al.,
2010) and PEMA.LiClO
4
(Amir et al., 2011).
Initially we must estimate the values of and
parameters. Based on Eq. 14, the parameter
originated from the second derivative of the interaction
energy of ion. We assumed the interaction energy
satisfies the Lennard-Jones potential Eq. 18 and 19:

6 12
0 0
E( ) ' 2
(
| | | |
= (
| |
\ \
(

(18)

So that:

2
0
'
36
kT

(19)

with ` is energy when the ions are separated by
0
.
This energy is not equal to the lowest energy in the pair
of atoms making a direct bonding. We derived based
on data of the lowest energy in the atomic bonding.
Since at large distances the dominant part in the
Lennard-Jones potential is the power six of the
distance, we speculated the lowest energy in case of ion
potential in the polymer electrolytes satisfies Eq. 20:

6
0
'
k k
| |

|
\

(20)

with is the distance of atoms making direct
bonding and is the lowest energy of the
corresponding direct bonding.
If N is the number of ions and V is the volume of
composite we have C = N/V. Let us estimate the
parameter for PVA containing Na ions. In this case,
N = m
Na
N
A
/MR
Na
, with MR
Na
is the atomic mass
of Na and N
A
is the Avogadro number. Furthermore,
V m
PVA
/
PVA
with
PVA
is the mass density of
PVA. Therefore Eq. 21 adn 22:

Na PVA PVA
A A
PVA Na Na
m C(wt%)
C N N
m MR 100 MR
| |
=
|
\
(21)

And:

1/ 3
Na
1/ 3 1/ 3
N
1 100MR 1
C C(wt%)
PVA A
| |
| =
|
\
(22)

The peak of conductivity occurs at a weight
fraction of ions at around 20%. The atomic mass of Na
is 23 and the density of PVA is around 1.26 g cm
3
.
Therefore, the estimated value for
0
5.3 10
-8
cm.
Assume the corresponding values for others ions are not
so far from this value so that we can use
0
5.3 10
-8

cm to estimate the parameter for other ions.
Several data on the interaction of atoms via
Lennard-Jones potential have been available. For
example, parameters of potential for interaction of
metal ions with oxygen atoms are /k = 1575.3 K and
= 0.34276 nm for Na
+
ion and /k = 2315.6K and
= 0.28517 nm for Li
+
ion (Zhen and Davies, 1983;
Lee and Rasaiah, 1996). Using these data into Eq.
(20) we obtained /k 115.5 K for Na ions and /k
56.2 K for Li ions.
The exponential factor controlling the ion
concentration is:

( ) ( )
( )
2 2
1/ 3 1/ 3 1/ 3 1/ 3
0 0 2
0
2/ 3
2
1/ 3 1/ 3 0
0
' 1
1/ C 1/ C 36 1/ C 1/ C
k T
' C
36 1/ C 1/ C
k T

If we use the unit of wt% for concentration, we
obtain an approximated estimation for parameter as
Eq. 23:

2/ 3
0
' C (wt%)
36
k T

(23)

Using /k 115.5 K for Na and /k 56.2 K for
Li, T = 300 K and C
0
20 wt% we obtain 102 for
Na and 50 for Li. Throughout the simulations we
selected the parameter within this range.
Am. J. Applied Sci., 9 (6): 946-954, 2012

950
The amorphous phase size can be estimated as
following. From the SEM images, the darker tone color
can be related to amorphous phase as suggested by
Zygado-Monikowska et al. (2007). SEM images of
grafted natural rubber containing LiF
4
as reported by
Ahmad el at. (2011a) showed darker tones in order of
submicrometer sizes (Ahmad et al., 2011b). Roiter and
Minko (2005) reported the appearances of real linear
polymer chains in liquid state on a surface as
recorded using an atomic force microscope have
contour length of about 204 nm (Roiter and Minko,
2005). This size might be related to the size of bulk
amorphous island of the polymer. Using a high
resolution solid state
13
C NMR, Zhang et al. (1992)
measured the amorphous phase size in polymer can
ranged from 2-30nm (Zhang et al., 1992). From these
reports, it is acceptable to assume values range
from 0.01-0.1 m. The diffusions coefficient of ions
in polymer is around 10
7
cm
2
s
1
(Klimuk and
Kuczajowska-Zadrozna, 2002; Stolwijk and Obeidi,
2004; Obeidi et al., 2004; 2005; Bracht et al., 1991).
Hirankumar et al. (2006) reported that the relaxation time
in polymer is around 10
5
s (Hirankumar et al., 2006).
From these data, we obtained the estimated values of
range from 0.1-10. In the following simulation we used
the values of parameter of around unity and the value
of parameter of around 100.

RESULTS

Figure 3 shows the comparison of experimental
data of conductivities of polymer electrolytes
(Bhargav et al., 2009; Aji et al., 2012; Hirankumar et
al., 2006; Mohamad et al., 2003; Noor et al., 2010;
Amir et al., 2011) and the fitting results. The fitting
parameters for each data are listed in the figure. In
the fitting results, the values of the volume fractions
of amorphous phase were selected so that the model
prediction fit the data properly. The selected volume
fractions are also displayed in the figure. It is clear
from Fig. 3a-d the fitting curves accurately fit the
experimental data for all polymer electrolytes.


(a) (b)


(c) (d)
Am. J. Applied Sci., 9 (6): 946-954, 2012

951

(e)

Fig. 3: Comparison of the experimental data (symbols) and the model predictions for polymer electrolytes of (a)
PVA.NaF, (b) PVA.LiOH, (c) PVA.AgNO
3
, (d) PEO.LiCF
3
SO
3
with ENR50 plasticizer and (e) PEMA.LiClO
4
.
The corresponding curves of dependence of amorphous phase on the ion concentration are also displayed

DISCUSSION

The selected prefactors conductivity
0
for all
polymer electrolytes were very close to the values
measured by many authors (Khiar and Arof, 2011;
Gong et al., 2008; Kang and Fang, 2004; Rajendran et
al., 2003; Kang et al., 2003; Xu et al., 2001). We also
see that the fraction of amorphous state increases with
the ion concentration and mostly saturates at high ion
concentration. These results are also consistent with the
observation of the XRD patterns of samples containing
different ion concentrations. Figure 4 shows the XRD
patterns of PVA.LiOH at different LiOH
concentrations. The XRD patterns confirmed the
dependence of the amorphous content on the ion
concentration (Aji et al., 2012). Reduced XRD intensity
is indicative of reduced crystallinity in the samples.
Similar observation has also been reported by other
authors in other polymer electrolyte systems (Ahmad et
al., 2011a; Fonseca et al., 2007). Ahmad et al. (2011b)
reported that in grafted natural rubber and poly (methyl
methacrylate), containing lithium tetrafluoroborate. The
degrees of crystallinity in systems of PCL-
biodegradable gel polymer electrolyte with LiClO
4
,
LiF
3
CSO
3
and LiBF
4
salts decreased nearly linear with
increasing the salt concentration (Ahmad et al., 2011a).
The increase in the amorphous content resulted
from inhibition of recrystallization of the host polymer
after the ions were dispersed. Ions located near the
polymer chains possess weak net electric charges that
could disturb the tendency of the chain to recrystallize
after heat treatment. Heat treatments are commonly
performed after addition of salts to polymer electrolytes
and consist of heating the polymer to near the melting
or glass transition temperature and slow cooling to
room temperature. This step increases the amorphous
phase content at room temperature, which is the
working temperature of most devices.
From the above results we selected a set of
conductivity parameters capable of predicting many
observed data reported by authors. The proposed
model was successful in describing the electrical
conductivity with two mechanisms in polymer
electrolyte systems.
Assume, the apparent activation energy for ion to
transport satisfies =
0
exp [E
a
/k T], by considering
Eq. 17 we can approximate the activation energy as
Eq. 24:

2/ 3 1/ 3 1/ 3 2
a a 0
E kT v (1/ C 1/ C )

( +

(24)

Using data in Fig. 4, we can calculate the effect
of salt or base weight fraction on the activation
energy for ion transport. Figure 5 shows the
activation energy of ions in several polymer
electrolytes as function of salt/base concentration.
The activation energy decreases with ion
concentration. At high ionic concentration, the
activation energies located at around 0.05 eV. This
activation energy corresponds to the activation energy
in amorphous phase. This value is comparable to what we
have reported previously when simulating the activation
energies of amorphous phase in various polymer
electrolytes of around 0.04 eV (Mikrajuddin et al.,
2000).
Am. J. Applied Sci., 9 (6): 946-954, 2012

952


Fig. 4: XRD patterns for (a) PVA powder, (b) PVA
membrane, (c) PVA.1wt%LiOH, (d) PVA.
3wt%LiOH, (e) PVA 5wt%LiOH, (f)
PVA.7wt%LiOH, (g) PVA.9wt%LiOH, (h)
PVA.10wt%LiOH and (i) LiOH powder



Fig. 5: Effect of salt or base weight fractions on the
activation energies for ion transport in the
polymer electrolytes

Furthermore, Mertens et al. (1999) reported, the
Vogel-Tamman-Fulcher activation energy of most
amorphous poly (ether-ester) s containing 1, 4, 7-
trioxanonyl main chain units at various LiClO
4

concentrations were mostly at around 8 kJ mol
1
or 0.08
eV (Mertens et al., 1999).

CONCLUSION

The new model introduced here succeeded to
explain the dependence of electrical conductivities of
various polymer electrolytes as function of ion
concentration. We only used a minimum number of
freely adjustable parameters to fit the data since some
parameters can be derived from experimental or
previously reported data. The model also predicted the
dependence of activation energies for ion transport that
were very close to those previously reported.

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